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  • 1
    In: Biogeosciences, Copernicus GmbH, Vol. 18, No. 24 ( 2021-12-22), p. 6547-6565
    Abstract: Abstract. The uptake of carbonyl sulfide (COS) by terrestrial plants is linked to photosynthetic uptake of CO2 as these gases partly share the same uptake pathway. Applying COS as a photosynthesis tracer in models requires an accurate representation of biosphere COS fluxes, but these models have not been extensively evaluated against field observations of COS fluxes. In this paper, the COS flux as simulated by the Simple Biosphere Model, version 4 (SiB4), is updated with the latest mechanistic insights and evaluated with site observations from different biomes: one evergreen needleleaf forest, two deciduous broadleaf forests, three grasslands, and two crop fields spread over Europe and North America. We improved SiB4 in several ways to improve its representation of COS. To account for the effect of atmospheric COS mole fractions on COS biosphere uptake, we replaced the fixed atmospheric COS mole fraction boundary condition originally used in SiB4 with spatially and temporally varying COS mole fraction fields. Seasonal amplitudes of COS mole fractions are ∼50–200 ppt at the investigated sites with a minimum mole fraction in the late growing season. Incorporating seasonal variability into the model reduces COS uptake rates in the late growing season, allowing better agreement with observations. We also replaced the empirical soil COS uptake model in SiB4 with a mechanistic model that represents both uptake and production of COS in soils, which improves the match with observations over agricultural fields and fertilized grassland soils. The improved version of SiB4 was capable of simulating the diurnal and seasonal variation in COS fluxes in the boreal, temperate, and Mediterranean region. Nonetheless, the daytime vegetation COS flux is underestimated on average by 8±27 %, albeit with large variability across sites. On a global scale, our model modifications decreased the modeled COS terrestrial biosphere sink from 922 Gg S yr−1 in the original SiB4 to 753 Gg S yr−1 in the updated version. The largest decrease in fluxes was driven by lower atmospheric COS mole fractions over regions with high productivity, which highlights the importance of accounting for variations in atmospheric COS mole fractions. The change to a different soil model, on the other hand, had a relatively small effect on the global biosphere COS sink. The secondary role of the modeled soil component in the global COS budget supports the use of COS as a global photosynthesis tracer. A more accurate representation of COS uptake in SiB4 should allow for improved application of atmospheric COS as a tracer of local- to global-scale terrestrial photosynthesis.
    Type of Medium: Online Resource
    ISSN: 1726-4189
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
    detail.hit.zdb_id: 2158181-2
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  • 2
    In: Biogeosciences, Copernicus GmbH, Vol. 20, No. 13 ( 2023-07-05), p. 2573-2594
    Abstract: Abstract. Carbonyl sulfide (COS) is a useful tracer to estimate gross primary production (GPP) because it shares part of the uptake pathway with CO2. COS is taken up in plants through hydrolysis, catalyzed by the enzyme carbonic anhydrase (CA), but is not released. The Simple Biosphere model version 4 (SiB4) simulates COS leaf uptake using a conductance approach. SiB4 applies the temperature response of the RuBisCo enzyme (used for photosynthesis) to simulate the COS leaf uptake, but the CA enzyme might respond differently to temperature. We introduce a new temperature response function for CA in SiB4, based on enzyme kinetics with an optimum temperature. Moreover, we determine Ball–Woodrow–Berry (BWB) model parameters for stomatal conductance (gs) using observation-based estimates of COS flux, GPP, and gs along with meteorological measurements in an evergreen needleleaf forest (ENF) and deciduous broadleaf forest (DBF). We find that CA has optimum temperatures of 20 ∘C (ENF) and 36 ∘C (DBF), which is lower than that of RuBisCo (45 ∘C), suggesting that canopy temperature changes can critically affect CA's catalyzation activity. Optimized values for the BWB offset parameter are similar to the original value (0.010 ± 0.003 mol m−2 s−1), and optimized values for the BWB slope parameter (ENF: 16.4, DBF: 11.4) are higher than the original value (9.0) at both sites. The optimization reduces prior errors on all parameters by more than 50 % at both stations. We apply the optimized gi and gs parameters in SiB4 site simulations, thereby improving the timing and peak of COS assimilation. In addition, we show that SiB4 underestimates the leaf humidity stress under conditions where high vapor pressure deficit (VPD) should limit gs in the afternoon, thereby overestimating gs. Furthermore, global COS biosphere sinks with optimized parameters show smaller COS uptake in regions where the air temperature is over 25 ∘C, mostly in the tropics, and larger uptake in regions where the temperature is below 25 ∘C. This change corresponds with reported deficiencies in the global COS fluxes, such as missing sinks at high latitudes and required sources in the tropics. Using our optimization and additional observations of COS uptake over various climate and plant types, we expect further improvements in global COS biosphere flux estimates.
    Type of Medium: Online Resource
    ISSN: 1726-4189
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2023
    detail.hit.zdb_id: 2158181-2
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  • 3
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 22, No. 4 ( 2022-02-25), p. 2569-2584
    Abstract: Abstract. The seasonality and interannual variability of terrestrial carbonyl sulfide (COS) fluxes are poorly constrained. We present the first easy-to-use parameterization for the net COS forest sink based on the longest existing eddy covariance record from a boreal pine forest, covering 32 months over 5 years. Fluxes from hourly to yearly scales are reported, with the aim of revealing controlling factors and the level of interannual variability. The parameterization is based on the photosynthetically active radiation, vapor pressure deficit, air temperature, and leaf area index. Wavelet analysis of the ecosystem fluxes confirmed earlier findings from branch-level fluxes at the same site and revealed a 3 h lag between COS uptake and air temperature maxima at the daily scale, whereas no lag between radiation and COS flux was found. The spring recovery of the flux after the winter dormancy period was mostly governed by air temperature, and the onset of the uptake varied by 2 weeks. For the first time, we report a significant reduction in ecosystem-scale COS uptake under a large water vapor pressure deficit in summer. The maximum monthly and weekly median COS uptake varied by 26 % and 20 % between years, respectively. The timing of the latter varied by 6 weeks. The fraction of the nocturnal uptake remained below 21 % of the total COS uptake. We observed the growing season (April–August) average net flux of COS totaling −58.0 g S ha−1 with 37 % interannual variability. The long-term flux observations were scaled up to evergreen needleleaf forests (ENFs) in the whole boreal region using the Simple Biosphere Model Version 4 (SiB4). The observations were closely simulated using SiB4 meteorological drivers and phenology. The total COS uptake by boreal ENFs was in line with a missing COS sink at high latitudes pointed out in earlier studies.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2022
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 4
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 5 ( 2021-03-08), p. 3507-3529
    Abstract: Abstract. Carbonyl sulfide (COS) has the potential to be used as a climate diagnostic due to its close coupling to the biospheric uptake of CO2 and its role in the formation of stratospheric aerosol. The current understanding of the COS budget, however, lacks COS sources, which have previously been allocated to the tropical ocean. This paper presents a first attempt at global inverse modelling of COS within the 4-dimensional variational data-assimilation system of the TM5 chemistry transport model (TM5-4DVAR) and a comparison of the results with various COS observations. We focus on the global COS budget, including COS production from its precursors carbon disulfide (CS2) and dimethyl sulfide (DMS). To this end, we implemented COS uptake by soil and vegetation from an updated biosphere model (Simple Biosphere Model – SiB4). In the calculation of these fluxes, a fixed atmospheric mole fraction of 500 pmol mol−1 was assumed. We also used new inventories for anthropogenic and biomass burning emissions. The model framework is capable of closing the COS budget by optimizing for missing emissions using NOAA observations in the period 2000–2012. The addition of 432 Gg a−1 (as S equivalents) of COS is required to obtain a good fit with NOAA observations. This missing source shows few year-to-year variations but considerable seasonal variations. We found that the missing sources are likely located in the tropical regions, and an overestimated biospheric sink in the tropics cannot be ruled out due to missing observations in the tropical continental boundary layer. Moreover, high latitudes in the Northern Hemisphere require extra COS uptake or reduced emissions. HIPPO (HIAPER Pole-to-Pole Observations) aircraft observations, NOAA airborne profiles from an ongoing monitoring programme and several satellite data sources are used to evaluate the optimized model results. This evaluation indicates that COS mole fractions in the free troposphere remain underestimated after optimization. Assimilation of HIPPO observations slightly improves this model bias, which implies that additional observations are urgently required to constrain sources and sinks of COS. We finally find that the biosphere flux dependency on the surface COS mole fraction (which was not accounted for in this study) may substantially lower the fluxes of the SiB4 biosphere model over strong-uptake regions. Using COS mole fractions from our inversion, the prior biosphere flux reduces from 1053 to 851 Gg a−1, which is closer to 738 Gg a−1 as was found by Berry et al. (2013). In planned further studies we will implement this biosphere dependency and additionally assimilate satellite data with the aim of better separating the role of the oceans and the biosphere in the global COS budget.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
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    detail.hit.zdb_id: 2069847-1
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  • 5
    In: Earth System Science Data, Copernicus GmbH, Vol. 15, No. 2 ( 2023-02-06), p. 579-605
    Abstract: Abstract. We present the CarbonTracker Europe High-Resolution (CTE-HR) system that estimates carbon dioxide (CO2) exchange over Europe at high resolution (0.1 × 0.2∘) and in near real time (about 2 months' latency). It includes a dynamic anthropogenic emission model, which uses easily available statistics on economic activity, energy use, and weather to generate anthropogenic emissions with dynamic time profiles at high spatial and temporal resolution (0.1×0.2∘, hourly). Hourly net ecosystem productivity (NEP) calculated by the Simple Biosphere model Version 4 (SiB4) is driven by meteorology from the European Centre for Medium-Range Weather Forecasts (ECMWF) Reanalysis 5th Generation (ERA5) dataset. This NEP is downscaled to 0.1×0.2∘ using the high-resolution Coordination of Information on the Environment (CORINE) land-cover map and combined with the Global Fire Assimilation System (GFAS) fire emissions to create terrestrial carbon fluxes. Ocean CO2 fluxes are included in our product, based on Jena CarboScope ocean CO2 fluxes, which are downscaled using wind speed and temperature. Jointly, these flux estimates enable modeling of atmospheric CO2 mole fractions over Europe. We assess the skill of the CTE-HR CO2 fluxes (a) to reproduce observed anomalies in biospheric fluxes and atmospheric CO2 mole fractions during the 2018 European drought, (b) to capture the reduction of anthropogenic emissions due to COVID-19 lockdowns, (c) to match mole fraction observations at Integrated Carbon Observation System (ICOS) sites across Europe after atmospheric transport with the Transport Model, version 5 (TM5) and the Stochastic Time-Inverted Lagrangian Transport (STILT), driven by ECMWF-IFS, and (d) to capture the magnitude and variability of measured CO2 fluxes in the city center of Amsterdam (the Netherlands). We show that CTE-HR fluxes reproduce large-scale flux anomalies reported in previous studies for both biospheric fluxes (drought of 2018) and anthropogenic emissions (COVID-19 pandemic in 2020). After applying transport of emitted CO2, the CTE-HR fluxes have lower median root mean square errors (RMSEs) relative to mole fraction observations than fluxes from a non-informed flux estimate, in which biosphere fluxes are scaled to match the global growth rate of CO2 (poor person's inversion). RMSEs are close to those of the reanalysis with the CTE data assimilation system. This is encouraging given that CTE-HR fluxes did not profit from the weekly assimilation of CO2 observations as in CTE. We furthermore compare CO2 concentration observations at the Dutch Lutjewad coastal tower with high-resolution STILT transport to show that the high-resolution fluxes manifest variability due to different emission sectors in summer and winter. Interestingly, in periods where synoptic-scale transport variability dominates CO2 concentration variations, the CTE-HR fluxes perform similarly to low-resolution fluxes (5–10× coarsened). The remaining 10 % of the simulated CO2 mole fraction differs by 〉2 ppm between the low-resolution and high-resolution flux representation and is clearly associated with coherent structures (“plumes”) originating from emission hotspots such as power plants. We therefore note that the added resolution of our product will matter most for very specific locations and times when used for atmospheric CO2 modeling. Finally, in a densely populated region like the Amsterdam city center, our modeled fluxes underestimate the magnitude of measured eddy covariance fluxes but capture their substantial diurnal variations in summertime and wintertime well. We conclude that our product is a promising tool for modeling the European carbon budget at a high resolution in near real time. The fluxes are freely available from the ICOS Carbon Portal (CC-BY-4.0) to be used for near-real-time monitoring and modeling, for example, as an a priori flux product in a CO2 data assimilation system. The data are available at https://doi.org/10.18160/20Z1-AYJ2 (van der Woude, 2022a).
    Type of Medium: Online Resource
    ISSN: 1866-3516
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2023
    detail.hit.zdb_id: 2475469-9
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  • 6
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 9, No. 11 ( 2016-11-01), p. 5293-5314
    Abstract: Abstract. Carbonyl sulfide (COS) has been suggested as a useful tracer for gross primary production as it is taken up by plants in a similar way as CO2. To explore and verify the application of this novel tracer, it is highly desired to develop the ability to perform continuous and high-precision in situ atmospheric measurements of COS and CO2. In this study we have tested a quantum cascade laser spectrometer (QCLS) for its suitability to obtain accurate and high-precision measurements of COS and CO2. The instrument is capable of simultaneously measuring COS, CO2, CO and H2O after including a weak CO absorption line in the extended wavelength range. An optimal background and calibration strategy was developed based on laboratory tests to ensure accurate field measurements. We have derived water vapor correction factors based on a set of laboratory experiments and found that for COS the interference associated with a water absorption line can dominate over the effect of dilution. This interference can be solved mathematically by fitting the COS spectral line separately from the H2O spectral line. Furthermore, we improved the temperature stability of the QCLS by isolating it in an enclosed box and actively cooling its electronics with the same thermoelectric chiller used to cool the laser. The QCLS was deployed at the Lutjewad atmospheric monitoring station (60 m; 6°21′ E, 53°24′ N; 1 m a.s.l.) in the Netherlands from July 2014 to April 2015. The QCLS measurements of independent working standards while deployed in the field showed a mean difference with the assigned cylinder value within 3.3 ppt COS, 0.05 ppm for CO2 and 1.7 ppb for CO over a period of 35 days. The different contributions to uncertainty in measurements of COS, CO2 and CO were summarized and the overall uncertainty was determined to be 7.5 ppt for COS, 0.23 ppm for CO2 and 3.3 ppb for CO for 1-minute data. A comparison of in situ QCLS measurements with those from concurrently filled flasks that were subsequently measured by the QCLS showed a difference of −9.7 ± 4.6 ppt for COS. Comparison of the QCLS with a cavity ring-down spectrometer showed a difference of 0.12 ± 0.77 ppm for CO2 and −0.9 ± 3.8 ppb for CO.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2016
    detail.hit.zdb_id: 2505596-3
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  • 7
    In: Journal of Geophysical Research: Atmospheres, American Geophysical Union (AGU), Vol. 128, No. 6 ( 2023-03-27)
    Abstract: The model‐observation mismatch suggests there is a missing source in the tropics and a missing sink in the high northern latitude in summer At northern latitude sites, the model spread in seasonal amplitude reaches 50 ppt compared to a mean seasonal amplitude of about 100 ppt The diurnal rectifier effect is small, decreasing the seasonal amplitude by up to 20% at continental sites
    Type of Medium: Online Resource
    ISSN: 2169-897X , 2169-8996
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 2023
    detail.hit.zdb_id: 710256-2
    detail.hit.zdb_id: 2016800-7
    detail.hit.zdb_id: 2969341-X
    SSG: 16,13
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  • 8
    Online Resource
    Online Resource
    Springer Science and Business Media LLC ; 2016
    In:  Boundary-Layer Meteorology Vol. 160, No. 3 ( 2016-9), p. 501-527
    In: Boundary-Layer Meteorology, Springer Science and Business Media LLC, Vol. 160, No. 3 ( 2016-9), p. 501-527
    Type of Medium: Online Resource
    ISSN: 0006-8314 , 1573-1472
    Language: English
    Publisher: Springer Science and Business Media LLC
    Publication Date: 2016
    detail.hit.zdb_id: 242879-9
    detail.hit.zdb_id: 1477639-X
    SSG: 16,13
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  • 9
    Online Resource
    Online Resource
    Proceedings of the National Academy of Sciences ; 2019
    In:  Proceedings of the National Academy of Sciences Vol. 116, No. 7 ( 2019-02-12), p. 2470-2475
    In: Proceedings of the National Academy of Sciences, Proceedings of the National Academy of Sciences, Vol. 116, No. 7 ( 2019-02-12), p. 2470-2475
    Abstract: Understanding climate controls on gross primary productivity (GPP) is crucial for accurate projections of the future land carbon cycle. Major uncertainties exist due to the challenge in separating GPP and respiration from observations of the carbon dioxide (CO 2 ) flux. Carbonyl sulfide (COS) has a dominant vegetative sink, and plant COS uptake is used to infer GPP through the leaf relative uptake (LRU) ratio of COS to CO 2 fluxes. However, little is known about variations of LRU under changing environmental conditions and in different phenological stages. We present COS and CO 2 fluxes and LRU of Scots pine branches measured in a boreal forest in Finland during the spring recovery and summer. We find that the diurnal dynamics of COS uptake is mainly controlled by stomatal conductance, but the leaf internal conductance could significantly limit the COS uptake during the daytime and early in the season. LRU varies with light due to the differential light responses of COS and CO 2 uptake, and with vapor pressure deficit (VPD) in the peak growing season, indicating a humidity-induced stomatal control. Our COS-based GPP estimates show that it is essential to incorporate the variability of LRU with environmental variables for accurate estimation of GPP on ecosystem, regional, and global scales.
    Type of Medium: Online Resource
    ISSN: 0027-8424 , 1091-6490
    RVK:
    RVK:
    Language: English
    Publisher: Proceedings of the National Academy of Sciences
    Publication Date: 2019
    detail.hit.zdb_id: 209104-5
    detail.hit.zdb_id: 1461794-8
    SSG: 11
    SSG: 12
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  • 10
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 17, No. 18 ( 2017-09-26), p. 11453-11465
    Abstract: Abstract. Nighttime vegetative uptake of carbonyl sulfide (COS) can exist due to the incomplete closure of stomata and the light independence of the enzyme carbonic anhydrase, which complicates the use of COS as a tracer for gross primary productivity (GPP). In this study we derived nighttime COS fluxes in a boreal forest (the SMEAR II station in Hyytiälä, Finland; 61°51′ N, 24°17′ E; 181 m a.s.l.) from June to November 2015 using two different methods: eddy-covariance (EC) measurements (FCOS-EC) and the radon-tracer method (FCOS-Rn). The total nighttime COS fluxes averaged over the whole measurement period were −6.8 ± 2.2 and −7.9 ± 3.8 pmol m−2 s−1 for FCOS-Rn and FCOS-EC, respectively, which is 33–38 % of the average daytime fluxes and 21 % of the total daily COS uptake. The correlation of 222Rn (of which the source is the soil) with COS (average R2  =  0.58) was lower than with CO2 (0.70), suggesting that the main sink of COS is not located at the ground. These observations are supported by soil chamber measurements that show that soil contributes to only 34–40 % of the total nighttime COS uptake. We found a decrease in COS uptake with decreasing nighttime stomatal conductance and increasing vapor-pressure deficit and air temperature, driven by stomatal closure in response to a warm and dry period in August. We also discuss the effect that canopy layer mixing can have on the radon-tracer method and the sensitivity of (FCOS-EC) to atmospheric turbulence. Our results suggest that the nighttime uptake of COS is mainly driven by the tree foliage and is significant in a boreal forest, such that it needs to be taken into account when using COS as a tracer for GPP.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2017
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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